Measurement of the activity and determination of the half-life of 225Ac at POLATOM.

A method for absolute measurements of the 225Ac activity in equilibrium with its progeny was developed. Measurements were performed using the triple-to-double coincidence ratio (TDCR) method in two different TDCR counters. The activity concentration of an 225Ac solution was determined and the solution was sent to the SIR system for a comparison. The half-life of 225Ac was determined by one of the TDCR counters and found to be 9.9150(63) days.

The next generation of current measurement for ionization chambers.

Re-entrant ionization chambers (ICs) are essential to radionuclide metrology and nuclear medicine for maintaining standards and measuring half-lives. The requirements of top-level metrology demand that systems must be precise and stable to 0.1 % over many years, and linear from 10-14 A to 10-8 A. Thus, laboratories depend on bespoke current measurement systems and often rely on sealed sources to generate reference currents. To maintain and improve present capabilities, metrologists need to overcome two looming challenges: ageing electronics and decreasing availability of sealed sources. Possible solutions using Ultrastable Low-Noise Current Amplifiers (ULCAs), resistive-feedback electrometers, and (quantum) single-electron pumps are reviewed. Broader discussions of IC design and methodology are discussed. ULCAs show promise and resistive-feedback systems which take advantage of standard resistor calibrations offer an alternative.

The first official measurement of 11C in the SIRTI.

In the summer of 2017, the Système International de Référence Transfer Instrument (SIRTI) of the Bureau International des Poids et Mesures (BIPM) was hosted by the National Research Council of Canada (NRC) in Ottawa, Canada. This SIRTI visit was unique in many aspects. It was the first visit of the SIRTI to Canada. NRC was the first National Metrological Institute (NMI) to perform comparisons of four isotopes (99mTc, 18F, 64Cu and 11C) during a single two-week period. Finally, this was the first official measurement of 11C in the SIRTI. The NRC had performed a primary standardization of 11C in February of 2017 and calibrated its Secondary Standard Ionizing Radiation Chamber System (SSIRCS) in preparation for the SIRTI comparison. Two primary Liquid Scintillation methods (CIEMAT/NIST and TDCR) were employed and the results agreed. The stock material was received from a local cyclotron in the form of a 11C-labelled sodium acetate (NaC2H3O2). Three ampoules were prepared for the purposes of comparison; one concentrated from the bulk material and two derived from a single dilution. Some inconsistency was evident due to a weighing problem for one of the ampoules containing the diluted solution, whose measurements were excluded from the analysis. The other two ampoules' results were consistent within their respective uncertainties. The SIRTI was very stable and the final BIPM report will detail the stability checks, performance and behaviour of the SIRTI during its measurement campaign in Canada. There is still no Key Comparison Reference Value (KCRV) for 11C as NRC is the first participant. However, during a test of the SIRTI at NPL in 2014, an equivalent SIRTI activity was measured as 9.87(5) kBq which was consistent with MonteCarlo predictions for 11C in the SIRTI of 9.867(15) kBq. The NRC SIRTI equivalent activity for 11C agrees within uncertainty with these results. This offers encouragement to other NMIs to request a 11C comparison given the consistency of experimental results from NRC and test results from the National Physical Laboratory, UK (NPL) and the BIPM. Finally a half-life measurement was determined from the NRC measurement of multiple half-lives of a 11C ampoule and was found to be 20.332(40)min. From the SIRTI measurements at NRC, the half-life was derived as 20.328(13) min. This is smaller but consistent with the DDEP recommended value of 20.361(23)min.

Activity measurements of the radionuclides 18F and 64Cu for the NIST, USA in the ongoing comparisons BIPM.RI(II)-K4.F-18 and BIPM.RI(II)-K4.Cu-64.

In 2016, comparisons of activity measurements of 18F and 64Cu using the Transfer Instrument of the International Reference System (SIRTI) took place at the National Institute of Standards and Technology (NIST, USA). This is the first SIRTI comparison for 64Cu. Ampoules containing about 27 kBq of 18F and 100 kBq of 64Cu solutions were measured in the SIRTI for about 5 and 1.5 half-lives, respectively. The NIST standardized the activity in the ampoules by ionization chamber measurements traceable to 4π(LS)ß-γ anticoincidence measurements. The comparisons, identifiers BIPM.RI(II)-K4.F-18 and BIPM.RI(II)-K4.Cu-64, are linked to the corresponding BIPM.RI(II)-K1.F-18 and BIPM.RI(II)-K1.Cu-64 comparisons and degrees of equivalence with the respective key comparison reference values have been evaluated. The NIST replaces its earlier degree of equivalence for 18F obtained in the frame of the CCRI(II)-K3.F-18 comparison in 2001.

Evidence against solar influence on nuclear decay constants.

The hypothesis that proximity to the Sun causes variation of decay constants at permille level has been tested and disproved. Repeated activity measurements of mono-radionuclide sources were performed over periods from 200 days up to four decades at 14 laboratories across the globe. Residuals from the exponential nuclear decay curves were inspected for annual oscillations. Systematic deviations from a purely exponential decay curve differ from one data set to another and are attributable to instabilities in the instrumentation and measurement conditions. The most stable activity measurements of alpha, beta-minus, electron capture, and beta-plus decaying sources set an upper limit of 0.0006% to 0.008% to the amplitude of annual oscillations in the decay rate. Oscillations in phase with Earth's orbital distance to the Sun could not be observed within a 10-6 to 10-5 range of precision. There are also no apparent modulations over periods of weeks or months. Consequently, there is no indication of a natural impediment against sub-permille accuracy in half-life determinations, renormalisation of activity to a distant reference date, application of nuclear dating for archaeology, geo- and cosmochronology, nor in establishing the SI unit becquerel and seeking international equivalence of activity standards.

Comparison of (18)F activity measurements at the VNIIM, NPL and the ENEA-INMRI using the SIRTI of the BIPM.

In 2014, the first three comparisons of activity measurements of (18)F were carried out at the VNIIM, NPL and the ENEA-INMRI using the BIPM's Transfer Instrument of the International Reference System. The transfer instrument and the NMIs primary measurement methods are briefly described. The degrees of equivalence with the key comparison reference value defined in the frame of the corresponding SIR comparison have been evaluated. World-wide consistency of activity measurements of (18)F is demonstrated.

Comparison of (99m)Tc activity measurements at the KRISS using the new SIRTI of the BIPM.

In 2010, a comparison of activity measurements of (99m)Tc was carried out at the KRISS using the BIPM's Transfer Instrument of the International Reference System (SIRTI). The transfer instrument and the KRISS coincidence measurement method are briefly described. The degrees of equivalence with the key comparison reference value and between the present KRISS result and the earlier participants in the SIRTI and SIR comparisons have been evaluated. World-wide consistency of activity measurements of (99m)Tc is demonstrated.

An approach based on the SIR measurement model for determining the ionization chamber efficiency curves, and a study of 65Zn and 201Tl photon emission intensities.

The measurement model used to determine ionization chamber efficiency curves accounts from the outset for impurity corrections and beta spectrum shapes. The curves are represented by exponentials of polynomials whose coefficients are adjusted using non-linear least-squares minimization. The curves are validated by comparing with SIR key comparison reference values (KCRVs) and other published curves. The associated covariance matrix is also evaluated. Deviations from model predictions for 65Zn and 201Tl using recommended nuclear data are studied.

Efficiency curve of the ionization chamber of the SIR.

The efficiency of the SIR ionization chamber versus photon energy has been obtained by an iterative method, starting from a few monoenergetic gamma-ray emitters. The relative standard uncertainty on the efficiency curve obtained is lower than 10(-2) above 65 keV. An efficiency curve for beta particles has been deduced in a similar manner, from measurements of (quasi-) pure beta emitters. The possible uses of the efficiency curve to identify inconsistent SIR data or discrepant decay scheme data are discussed.

Standardization and decay data of 237Np.

This paper reports contributions from participants in the EUROMET project (No. 416) which was entitled "237Np research into problems relating to purification, characterization and standardization". Primary standardizations were made by the defined low solid angle, coincidence, 4pi alpha, 2pi alpha and liquid scintillation counting methods. Secondary standardizations were made with calibrated gamma-ray spectrometers. Absolute X-ray, gamma-ray and alpha-particle emission probabilities were also determined. The results for the successful conclusion of both primary and secondary standardization are presented together with the values for alpha-particle and gamma-ray emission probabilities determined in this exercise. Several significant inconsistencies remain with the gamma-ray emission probabilities, and these are highlighted.

Influence of radioactive impurities on SIR measurements

The correction usually applied to an SIR measurement in the presence of a gamma-ray emitting impurity is presented and explained. The method of calibration of a Ge(Li) spectrometer is briefly described. It is used to look for impurities when SIR measurements show inconsistencies. An example is presented where a 103Ru impurity was discovered in a 99Mo solution. The correction applied compensates for the decrease of around 0.2% per day observed in the SIR measurements of this 99Mo ampoule.